Dopant Engineering in Perovskite Cathodes for Efficient <scp> CO ₂ </scp> Electrolysis

Electrochemical carbon dioxide reduction reaction (CO 2 RR), powered by advanced technologies such as solid oxide electrolysis cells (SOEC), is a promising method to convert CO 2 into valuable carbon‐based products using renewable electricity. The high chemical stability of CO 2 requires catalysts to exhibit both high activity and stable electrocatalytic performance. However, catalysts that deliver high performance in CO 2 RR are rare and still require further improvement. Here, we report a strategy that can efficiently enhance catalyst activity through Zn doping, which introduces active frustrated Lewis pairs (FLP) to improve the catalyst's ability to activate small molecules. A high current density of −1.85 A cm −2 at 800 °C under a bias voltage of 1.5 V was achieved using the Sr 2 Fe 0.8 Zn 0.2 MoO 6‐δ (SFZn 0.2 M) cathode with pure CO 2 feeding gas, surpassing previously reported results for perovskite oxide cathodes. This SOEC device also demonstrates excellent stability, with negligible degradation over tests lasting up to 110 h.